Non-Fickian (or anomalous) transport of contaminants has been observed at field and laboratory scales in a wide variety of porous and fractured geological formations. Over many years a basic challenge to the hydrology community has been to develop a theoretical framework that quantitatively accounts for this widespread phenomenon. Recently, continuous time random walk (CTRW) formulations have been demonstrated to provide general and effective means to quantify non-Fickian transport. We introduce and develop the CTRW framework from its conceptual picture of transport through its mathematical development to applications relevant to laboratory- and field-scale systems. The CTRW approach contrasts with ones used extensively on the basis of the advection-dispersion equation and use of upscaling, volume averaging, and homogenization. We examine the underlying assumptions, scope, and differences of these approaches, as well as stochastic formulations, relative to CTRW. We argue why these methods have not been successful in fitting actual measurements. The CTRW has now been developed within the framework of partial differential equations and has been generalized to apply to nonstationary domains and interactions with immobile states (matrix effects). We survey models based on multirate mass transfer (mobile-immobile) and fractional derivatives and show their connection as subsets within the CTRW framework.